Cristin-resultat-ID: 1038276
Sist endret: 14. august 2013, 13:41
NVI-rapporteringsår: 2013
Resultat
Vitenskapelig artikkel
2013

Reactive scattering of H-2 from Cu(100): Comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experiment

Bidragsytere:
  • L. Sementa
  • M. Wijzenbroek
  • B.J. van Kolck
  • M.F. Somers
  • A. Al-Halabi
  • H.F. Busnengo
  • mfl.

Tidsskrift

Journal of Chemical Physics
ISSN 0021-9606
e-ISSN 1089-7690
NVI-nivå 1

Om resultatet

Vitenskapelig artikkel
Publiseringsår: 2013
Volum: 138
Hefte: 4

Importkilder

Isi-ID: 000314725900056
Scopus-ID: 2-s2.0-84873584780

Beskrivelse Beskrivelse

Tittel

Reactive scattering of H-2 from Cu(100): Comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experiment

Sammendrag

We present new experimental and theoretical results for reactive scattering of dihydrogen from Cu(100). In the new experiments, the associative desorption of H2 is studied in a velocity resolved and final rovibrational state selected manner, using time-of-flight techniques in combination with resonance-enhanced multi-photon ionization laser detection. Average desorption energies and rotational quadrupole alignment parameters were obtained in this way for a number of (v = 0, 1) rotational states, v being the vibrational quantum number. Results of quantum dynamics calculations based on a potential energy surface computed with a specific reaction parameter (SRP) density functional, which was derived earlier for dihydrogen interacting with Cu(111), are compared with the results of the new experiments and with the results of previous molecular beam experiments on sticking of H2 and on rovibrationally elastic and inelastic scattering of H2 and D2 from Cu(100). The calculations use the Born-Oppenheimer and static surface approximations. With the functional derived semi-empirically for dihydrogen + Cu(111), a chemically accurate description is obtained of the molecular beam experiments on sticking of H2 on Cu(100), and a highly accurate description is obtained of rovibrationally elastic and inelastic scattering of D2 from Cu(100) and of the orientational dependence of the reaction of (v = 1, j = 2 − 4) H2 on Cu(100). This suggests that a SRP density functional derived for H2 interacting with a specific low index face of a metal will yield accurate results for H2 reactively scattering from another low index face of the same metal, and that it may also yield accurate results for H2 interacting with a defected (e.g., stepped) surface of that same metal, in a system of catalytic interest. However, the description that was obtained of the average desorption energies, of rovibrationally elastic and inelastic scattering of H2 from Cu(100), and of the orientational dependence of reaction of (v = 0, j = 3 − 5, 8) H2 on Cu(100) compares less well with the available experiments. More research is needed to establish whether more accurate SRP-density functional theory dynamics results can be obtained for these observables if surface atom motion is added to the dynamical model. The experimentally and theoretically found dependence of the rotational quadrupole alignment parameter on the rotational quantum number provides evidence for rotational enhancement of reaction at low translational energies.

Bidragsytere

L. Sementa

  • Tilknyttet:
    Forfatter
    ved Consiglio Nazionale delle Ricerche
  • Tilknyttet:
    Forfatter
    ved Universiteit Leiden

M. Wijzenbroek

  • Tilknyttet:
    Forfatter
    ved Universiteit Leiden

B.J. van Kolck

  • Tilknyttet:
    Forfatter
    ved Universiteit Leiden

M.F. Somers

  • Tilknyttet:
    Forfatter
    ved Universiteit Leiden

A. Al-Halabi

  • Tilknyttet:
    Forfatter
    ved Universiteit Leiden
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